Existence of multi-radical and closed-shell semiconducting states in post-graphene organic Dirac materials.
Existence of multi-radical and closed-shell semiconducting states in post-graphene organic Dirac materials.
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DOI：
10.1038/s41467-017-01977-4
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发表时间：
2017-12-05
影响因子：
16.6
通讯作者：
Bromley ST
中科院分区：
文献类型：
--
作者：
Alcón I;Viñes F;Moreira IPR;Bromley ST
后石墨烯有机狄拉克（PGOD）材料是由π-共轭连接体间隔的三重键合sp2碳节点的有序二维网络。PGOD材料是石墨烯的天然化学延伸，有望具有更广泛的性能和应用。实验上实现的分子的基础上两个PGOD节点表现出双稳定的封闭壳层/多自由基的字符，可以理解通过竞争刘易斯共振形式。在这里，遵循相同的原理，我们预测PGOD材料中应该可以达到类似的状态，我们使用准确的密度泛函理论计算证实了这一点。虽然对于石墨烯，半金属状态总是占主导地位，但对于PGOD材料，这种状态相对于通过对称性破缺稳定的开壳多自由基和/或闭壳状态变得边缘亚稳定，与类似的分子系统一致。这些后一种状态是半导体的，增加了PGOD材料作为未来有机纳米电子学和自旋电子学的高度可调平台的潜在用途。石墨烯中带隙可控性的缺乏严重限制了其在纳米电子学中的应用。在这里，作者预测，后石墨烯有机狄拉克材料应该允许石墨烯类半金属性和多自由基和/或闭壳半导体状态之间的特殊电子可调性。
Post-graphene organic Dirac (PGOD) materials are ordered two-dimensional networks of triply bonded sp 2 carbon nodes spaced by π-conjugated linkers. PGOD materials are natural chemical extensions of graphene that promise to have an enhanced range of properties and applications. Experimentally realised molecules based on two PGOD nodes exhibit a bi-stable closed-shell/multi-radical character that can be understood through competing Lewis resonance forms. Here, following the same rationale, we predict that similar states should be accessible in PGOD materials, which we confirm using accurate density functional theory calculations. Although for graphene the semimetallic state is always dominant, for PGOD materials this state becomes marginally meta-stable relative to open-shell multi-radical and/or closed-shell states that are stabilised through symmetry breaking, in line with analogous molecular systems. These latter states are semiconducting, increasing the potential use of PGOD materials as highly tuneable platforms for future organic nano-electronics and spintronics. The lack of band gap controllability in graphene severely restricts its use in nanoelectronics. Here, the authors predict that post-graphene organic Dirac materials should allow for exceptional electronic tunability between graphene-like semimetallicity and multi-radical and/or closed-shell semiconducting states.
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影响因子：
4.6
作者：
Dutta S;Wakabayashi K
通讯作者：
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作者：
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影响因子：
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作者：
IIJIMA, S
通讯作者：
IIJIMA, S